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arXiv:2211.01360 · Physical review. B./Physical review. B

High-field quantum spin liquid transitions and angle-field phase diagram of the Kitaev magnet α−RuCl3

Han Li, Wei Li, Gang Su

Published Mar 10, 2023• 5 citations
arXivHTMLPDF

Abstract

The pursuit of quantum spin liquid (QSL) in the Kitaev honeycomb magnets has drawn intensive attention recently. In particular, $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$ has been widely recognized as a promising candidate for the Kitaev QSL. Although the compound exhibits an antiferromagnetic order under zero field, it is believed to be endowed with fractionalized excitations and can be driven to the QSL phase by magnetic fields. Here, based on a realistic $K\text{\ensuremath{-}}J\text{\ensuremath{-}}\mathrm{\ensuremath{\Gamma}}\text{\ensuremath{-}}{\mathrm{\ensuremath{\Gamma}}}^{\ensuremath{'}}$ model for $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$, we exploit the exponential tensor renormalization group approach to explore the phase diagram of the compound under magnetic fields. We calculate the thermodynamic quantities, including the specific heat, Gr\"uneisen parameter, magnetic torque, magnetotropic susceptibility, and so on, under a magnetic field with a tilting angle $\ensuremath{\theta}$ to the ${c}^{*}$-axis perpendicular to the honeycomb plane. We find an extended QSL in the angle-field phase diagram determined with thermodynamic responses. The gapless nature of such field-induced QSL is identified from the specific heat and entropy data computed down to very low temperatures. The present study provides guidance for future high-field experiments for the QSL in $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$ and other candidate Kitaev magnets.

DOI
10.1103/physrevb.107.115124

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The pursuit of quantum spin liquid (QSL) in the Kitaev honeycomb magnets has drawn intensive attention recently. In particular, \ensuremathα\ensuremath-RuCl3\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}\ensuremathα\ensuremath-RuCl3​ has been widely recognized as a promising candidate for the Kitaev QSL. Although the compound exhibits an antiferromagnetic order under zero field, it is believed to be endowed with fractionalized excitations and can be driven to the QSL phase by magnetic fields. Here, based on a realistic K\ensuremath-J\ensuremath-\ensuremathΓ\ensuremath-\ensuremathΓ\ensuremath′K\text{\ensuremath{-}}J\text{\ensuremath{-}}\mathrm{\ensuremath{\Gamma}}\text{\ensuremath{-}}{\mathrm{\ensuremath{\Gamma}}}^{\ensuremath{'}}K\ensuremath-J\ensuremath-\ensuremathΓ\ensuremath-\ensuremathΓ\ensuremath′ model for \ensuremathα\ensuremath-RuCl3\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}\ensuremathα\ensuremath-RuCl3​, we exploit the exponential tensor renormalization group approach to explore the phase diagram of the compound under magnetic fields. We calculate the thermodynamic quantities, including the specific heat, Gr"uneisen parameter, magnetic torque, magnetotropic susceptibility, and so on, under a magnetic field with a tilting angle \ensuremathθ\ensuremath{\theta}\ensuremathθ to the c∗{c}^{*}c∗-axis perpendicular to the honeycomb plane. We find an extended QSL in the angle-field phase diagram determined with thermodynamic responses. The gapless nature of such field-induced QSL is identified from the specific heat and entropy data computed down to very low temperatures. The present study provides guidance for future high-field experiments for the QSL in \ensuremathα\ensuremath-RuCl3\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}\ensuremathα\ensuremath-RuCl3​ and other candidate Kitaev magnets.
Abstract Pursuing the exotic quantum spin liquid (QSL) state in the Kitaev material α-RuCl3 has intrigued great research interest recently. A fascinating question is on the possible existence of a field-induced QSL phase in this compound. Here we perform high-field magnetization measurements of α-RuCl3 up to 102 T employing the non-destructive and destructive pulsed magnets. Under the out-of-plane field along the c* axis (i.e., perpendicular to the honeycomb plane), two quantum phase transitions are uncovered at respectively 35 T and about 83 T, between which lies an intermediate phase as the predicted QSL. This is in sharp contrast to the case with in-plane fields, where a single transition is found at around 7 T and the intermediate QSL phase is absent instead. By measuring the magnetization data with fields tilted from the c* axis up to 90° (i.e., in-plane direction), we obtain the field-angle phase diagram that contains the zigzag, paramagnetic, and QSL phases. Based on the K-J-Γ- Γ′{{{\Gamma }}}^{{\prime} }Γ′ Γ ′ model for α-RuCl3 with a large Kitaev term we perform density matrix renormalization group simulations and reproduce the quantum phase diagram in excellent agreement with experiments.
Recent experimental evidence for a field-induced quantum spin liquid (QSL) in ααα-RuCl3_33​ calls for an understanding for the ground state of honeycomb Kitaev model under a magnetic field. In this work we address the nature of an enigmatic gapless paramagnetic phase in the antiferromagnetic Kitave model, under an intermediate magnetic field perpendicular to the plane. Combining theoretical and numerical efforts, we identify this gapless phase as a U(1)U(1)U(1) QSL with spinon Fermi surfaces. We also reveal the nature of continuous quantum phase transitions involving this U(1)U(1)U(1) QSL, and obtain a phase diagram of the Kitaev model as a function of bond anisotropy and perpendicular magnetic field.
The possible existence of a quantum spin liquid (QSL) phase, an exotic state of matter with long-range quantum entanglement and fractionalized excitations, in ααα-RuCl3_33​ has sparked widespread interests in exploring QSLs in various Kitaev models under magnetic fields. Recently, a KKK-JJJ-ΓΓΓ-Γ′Γ'Γ′ model has been proposed to accurately describe the compound by fitting the measured thermodynamic data, where JJJ is Heisenberg interaction, and ΓΓΓ, Γ′Γ'Γ′ are off-diagonal exchanges on top of the dominant Kitaev coupling KKK. Based on this effective model, an intermediate QSL phase in presence of an out-of-plane fields along the [111][1 1 1][111] direction, between the low-field zigzag order and high-field polarized phase, has been predicted. By combining density matrix renormalization group (DMRG), exponential tensor renormalization group (XTRG), and variational Monte Carlo (VMC) calculations, we address the nature of this QSL phase in the honeycomb KKK-JJJ-ΓΓΓ-Γ′Γ'Γ′ model under the [111][1 1 1][111]-direction field. Our DMRG calculations find the algebraic-like decay of spin correlation function, the finite spin scalar chiral order, and lattice nematic order. Together with the XTRG results of power-law specific heat at low temperature, our findings naturally suggest a gapless nematic chiral spin liquid. On the other hand, our VMC study finds a gapped nematic chiral spin liquid with the variational energy very close to that obtained in DMRG. As VMC finds a very small gap that is beyond the current resolution of both ground-state DMRG and finite-temperature XTRG calculations on finite-width cylinders, we resort the full clarification for the nature of the intermediate QSL to future studies. Lastly, we discuss the implications of our results to the recent experiment on ααα-RuCl3_33​ and the QSL-like phase in a similar KKK-ΓΓΓ-Γ′Γ'Γ′ model.
Abstract The frustrated magnet α-RuCl3 constitutes a fascinating quantum material platform that harbors the intriguing Kitaev physics. However, a consensus on its intricate spin interactions and field-induced quantum phases has not been reached yet. Here we exploit multiple state-of-the-art many-body methods and determine the microscopic spin model that quantitatively explains major observations in α-RuCl3, including the zigzag order, double-peak specific heat, magnetic anisotropy, and the characteristic M-star dynamical spin structure, etc. According to our model simulations, the in-plane field drives the system into the polarized phase at about 7 T and a thermal fractionalization occurs at finite temperature, reconciling observations in different experiments. Under out-of-plane fields, the zigzag order is suppressed at 35 T, above which, and below a polarization field of 100 T level, there emerges a field-induced quantum spin liquid. The fractional entropy and algebraic low-temperature specific heat unveil the nature of a gapless spin liquid, which can be explored in high-field measurements on α-RuCl3.
Abstract The frustrated magnetα-RuCl3constitutes a fascinating quantum material platform that harbors the intriguing Kitaev physics. However, a consensus on its intricate spin interactions and field-induced quantum phases has not been reached yet. Here we exploit multiple state-of-the-art many-body methods and determine the microscopic spin model that quantitatively explains major observations inα-RuCl3, including the zigzag order, double-peak specific heat, magnetic anisotropy, and the characteristic M-star dynamical spin structure, etc. According to our model simulations, the in-plane field drives the system into the polarized phase at about 7 T and a thermal fractionalization occurs at finite temperature, reconciling observations in different experiments. Under out-of-plane fields, the zigzag order is suppressed at 35 T, above which, and below a polarization field of 100 T level, there emerges a field-induced quantum spin liquid. The fractional entropy and algebraic low-temperature specific heat unveil the nature of a gapless spin liquid, which can be explored in high-field measurements onα-RuCl3.
Measurements of the magnetic Gr\"uneisen parameter (${\mathrm{\ensuremath{\Gamma}}}_{B}$) and specific heat on the Kitaev material candidate $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$ are used to access in-plane field and temperature dependence of the entropy up to 12 T and down to 1 K. No signatures corresponding to phase transitions are detected beyond the boundary of the magnetically ordered region, but only a shoulderlike anomaly in ${\mathrm{\ensuremath{\Gamma}}}_{B}$, involving an entropy increment as small as ${10}^{\ensuremath{-}5}R\mathrm{log}2$. These observations put into question the presence of a phase transition between the purported quantum spin liquid and the field-polarized state of $\ensuremath{\alpha}\text{\ensuremath{-}}{\mathrm{RuCl}}_{3}$. We show theoretically that at low temperatures ${\mathrm{\ensuremath{\Gamma}}}_{B}$ is sensitive to crossings in the lowest excitations within gapped phases, and identify the measured shoulderlike anomaly as being of such origin. Exact diagonalization calculations demonstrate that the shoulderlike anomaly can be reproduced in extended Kitaev models that gain proximity to an additional phase at finite field without entering it. We discuss manifestations of this proximity in other measurements.